mass spectrometry; DNA; photodetachment; UV; visible; spectroscopy; fragmentation; noncovalent
Abstract :
[en] Double stranded DNA multiply charged anions coupled to chromophores were subjected to UV-Vis photoactivation. in a quadrupole ion trap mass spectrometer. The chromophores included noncovalently bound minor groove binders (activated in the near UV), noncovalently bound intercalators (activated with visible light), and covalently linked fluorophores and quenchers (activated at their maximum absorption wavelength). We found that the activation of only chromophores having long fluorescence lifetimes did result in efficient electron photodetachment from the DNA complexes. In the case of ethidium-dsDNA complex excited at 500 nm, photodetachment is a multiphoton process. The MS3 fragmentation of radicals produced by photodetachment at lambda = 260 nm (DNA excitation) and by photodetachment at lambda > 300 nm (chromophore excitation) were compared. The radicals keep no memory of the way they were produced. A weakly bound noncovalent ligand (m-amsacrine) allowed probing experimentally that a fraction of the electronic internal energy was converted into vibrational internal energy. This fragmentation channel was used to demonstrate that excitation of the quencher DABSYL resulted in internal conversion, unlike the fluorophore 6-FAM. Altogether, photodetachment of the DNA complexes upon chromophore excitation can be interpreted by the following mechanism: (1) ligands with sufficiently long excited-state lifetime undergo resonant two-photon excitation to reach the level of the DNA excited states, then (2) the excited-state must be coupled to the DNA excited states for photodetachment to occur. Our experiments also pave the way towards photodissociation probes of biomolecule conformation in the gas-phase by Forster resonance energy transfer (FRET).
Disciplines :
Physics Chemistry
Author, co-author :
Gabelica, Valérie ; Université de Liège - ULiège > Département de Chimie (Sciences) > Chimie physique, spectrométrie de masse
Rosu, Frédéric ; Université de Liège - ULiège > Département de Chimie (Sciences) > Chimie physique, spectrométrie de masse
De Pauw, Edwin ; Université de Liège - ULiège > Département de Chimie (Sciences) > Chimie physique, spectrométrie de masse
Antoine, Rodolphe; Université Lyon 1 et CNRS > Laboratoire de Spectrométrie Ionique et Moléculaire - LASIM
Tabarin, Thibault; Université Lyon 1 et CNRS > Laboratoire de Spectrométrie Ionique et Moléculaire - LASIM
Broyer, Michel; Université Lyon 1 et CNRS > Laboratoire de Spectrométrie Ionique et Moléculaire - LASIM
Dugourd, Philippe; Université Lyon 1 et CNRS > Laboratoire de Spectrométrie Ionique et Moléculaire - LASIM
Language :
English
Title :
Electron photodetachment dissociation of DNA anions with covalently or noncovalently bound chromophores
Publication date :
2007
Journal title :
Journal of the American Society for Mass Spectrometry
ISSN :
1044-0305
eISSN :
1879-1123
Publisher :
Elsevier Science, New York, United States - New York
Volume :
18
Issue :
11
Pages :
1990-2000
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE]
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